Consecutive Ligand-Based Electron Transfer in New Molecular Copper-Based Water Oxidation Catalysts.
Angew Chem Int Ed Engl
; 60(34): 18639-18644, 2021 Aug 16.
Article
em En
| MEDLINE
| ID: mdl-34015172
ABSTRACT
Water oxidation to dioxygen is one of the key reactions that need to be mastered for the design of practical devices based on water splitting with sunlight. In this context, water oxidation catalysts based on first-row transition metal complexes are highly desirable due to their low cost and their synthetic versatility and tunability through rational ligand design. A new family of dianionic bpy-amidate ligands of general formula H2 LNn- (LN is [2,2'-bipyridine]-6,6'-dicarboxamide) substituted with phenyl or naphthyl redox non-innocent moieties is described. A detailed electrochemical analysis of [(L4)Cu]2- (L4=4,4'-(([2,2'-bipyridine]-6,6'-dicarbonyl)bis(azanediyl))dibenzenesulfonate) at pHâ
11.6 shows the presence of a large electrocatalytic wave for water oxidation catalysis at an η=830â
mV. Combined experimental and computational evidence, support an all ligand-based process with redox events taking place at the aryl-amide groups and at the hydroxido ligands.
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Coleções:
01-internacional
Base de dados:
MEDLINE
Idioma:
En
Revista:
Angew Chem Int Ed Engl
Ano de publicação:
2021
Tipo de documento:
Article